After the tour, the group went right back into the studio, cutting the Dance to the Underground EP, signaling a shift in direction for Radio 4. The new EP focused on adding a more funky sound and some electronics, a path they would continue on for the next album.

Armed with a new focus to make a more upbeat, dance-y, funky record, Radio 4 hit the studio in NY with production duo DFA, known for producing electronic acts like UNKLE and David Holmes as well as dance rock bands The Rapture and Primal Scream. For 2001's Gotham!, the band achieved a more unique sound consisting of many layers of guitar licks, electronic beats, blips, squeaks, claps, and keyboards. Lyrically, the record was a tribute to New York City, appropriately fitting their New York sound. Since the album was recorded before the tragedies of September 11, 2001, their music would have even more meaning. With Gotham!, the group had come up with a winning sound that would create a nationwide buzz in indie rock circles, and would even get indie rock heavyweights The Faint to invite them along on their European tour.